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Towards wafer-size graphene layers by atmospheric pressure graphitization of silicon carbide

Abstract

Graphene, a single monolayer of graphite, has recently attracted considerable interest owing to its novel magneto-transport properties1,2,3, high carrier mobility and ballistic transport up to room temperature4. It has the potential for technological applications as a successor of silicon in the post Moore’s law era5,6,7, as a single-molecule gas sensor8, in spintronics9,10,11, in quantum computing12 or as a terahertz oscillator13. For such applications, uniform ordered growth of graphene on an insulating substrate is necessary. The growth of graphene on insulating silicon carbide (SiC) surfaces by high-temperature annealing in vacuum was previously proposed to open a route for large-scale production of graphene-based devices5,6. However, vacuum decomposition of SiC yields graphene layers with small grains (30–200 nm; refs 14–16). Here, we show that the ex situ graphitization of Si-terminated SiC(0001) in an argon atmosphere of about 1 bar produces monolayer graphene films with much larger domain sizes than previously attainable. Raman spectroscopy and Hall measurements confirm the improved quality of the films thus obtained. High electronic mobilities were found, which reach μ=2,000 cm 2 V−1 s−1 at T=27 K. The new growth process introduced here establishes a method for the synthesis of graphene films on a technologically viable basis.

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Figure 1: Morphological changes of 6H–SiC(0001) during graphene growth.
Figure 2: Atomic and electronic structure of ex-situ-grown monolayer graphene.

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Acknowledgements

We thank F. El Gabaly for assistance with the LEEM measurements and M. Gick for help with the sample preparation. We gratefully acknowledge support by the DFG under contract SE 1087/5-1, contract WE 4542-5-1, and within the Cluster of Excellence ‘Engineering of Advanced Materials’ (www.eam.uni-erlangen.de) at the Friedrich-Alexander-Universität Erlangen-Nürnberg, by BaCaTeC, and by the BMBF under contract 05 ES3XBA/5. A part of the work was carried out at Sandia National Laboratories, a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin company, for the United States Department of Energy, Office of Basic Energy Sciences, Division of Materials Science and Engineering, under Contract No. DE-AC04-94AL85000. The work carried out at the Advanced Light Source was supported by the Director, Office of Science, Office of Basic Energy Sciences, of the US Department of Energy under Contract No. DE-AC03-76SF00098.

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Contributions

K.V.E. developed the growth process of large-area graphene with the help of S.A.R. AFM measurements were done by K.V.E. and T.O. T.O. and A.S. carried out the LEEM measurements with the help of G.K. Photoelectron spectroscopy measurements were carried out by K.V.E., T.S., A.B., J.L.M., E.R. and K.H. J.J., D.W. and H.B.W carried out lithography and electrical measurements. J.R. carried out Raman measurements. T.S., K.V.E. and L.L. wrote the manuscript with revision and input from all other co-authors.

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Correspondence to Thomas Seyller.

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Emtsev, K., Bostwick, A., Horn, K. et al. Towards wafer-size graphene layers by atmospheric pressure graphitization of silicon carbide. Nature Mater 8, 203–207 (2009). https://doi.org/10.1038/nmat2382

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